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Atmospheric Chemistry and Physics An interactive open-access journal of the European Geosciences Union
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https://doi.org/10.5194/acp-2020-619
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-2020-619
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.

  06 Jul 2020

06 Jul 2020

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This preprint is currently under review for the journal ACP.

Atmospheric Evolution of Emissions from a Boreal Forest Fire: The Formation of Highly-Functionalized Oxygen-, Nitrogen-, and Sulfur-Containing Compounds

Jenna C. Ditto1, Megan He1, Tori N. Hass-Mitchell1, Samar G. Moussa2, Katherine Hayden2, Shao-Meng Li2, John Liggio2, Amy Leithead2, Patrick Lee2, Michael J. Wheeler2, Jeremy J. B. Wenztell2, and Drew R. Gentner1,3 Jenna C. Ditto et al.
  • 1Department of Chemical and Environmental Engineering, Yale University, New Haven, CT, 06511, USA
  • 2Air Quality Research Division, Environment and Climate Change Canada, Toronto, Ontario M3H 5T4, Canada
  • 3Solutions for Energy, Air, Climate and Health (SEARCH), School of the Environment, Yale University, New Haven CT 0651, USA

Abstract. Forest fires are major contributors of reactive gas- and particle-phase organic compounds to the atmosphere. We used offline high resolution tandem mass spectrometry to perform a molecular-level speciation of evolving gas- and particle-phase compounds sampled via aircraft from a boreal forest fire in Saskatchewan, Canada. We observed diverse multifunctional compounds containing oxygen, nitrogen, and sulfur (CHONS), whose structure, formation, and impacts are understudied. The abundance of particle-phase CHONS species increased with plume age, from 19 % to 40 % of the relative abundance of observed functionalized OA over the first 4 hours of downwind transport. The relative contribution of particle-phase sulfide functional groups increased with age from 4 % to 40 % of observed OA abundance, and were present in up to 75 % of CHONS compounds. The increases in sulfides were accompanied by increases in ring-bound nitrogen, and both increased together with CHONS prevalence. A complex mixture of intermediate- and semi-volatile gas-phase organic sulfur species was emitted from the fire and depleted downwind, representing potential precursors to particle-phase CHONS compounds. These results demonstrate CHONS formation from nitrogen/oxygen-containing biomass burning emissions in the presence of reduced sulfur species, and highlight chemical pathways that may also be relevant in situations with elevated levels of nitrogen and sulfur emissions from residential biomass burning and fossil fuel use (e.g. coal), respectively.

Jenna C. Ditto et al.

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Jenna C. Ditto et al.

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Short summary
Forest fires are an important source of reactive organic gases and aerosols to the atmosphere. We analyzed organic aerosols collected from an aircraft above a boreal forest fire, and reported an increasing contribution from compounds containing oxygen, nitrogen, and sulfur with plume age, with sulfide and ring-bound nitrogen functionality. Our results demonstrated chemistry that is important in biomass burning but also in urban/developing regions with high local nitrogen/sulfur emissions.
Forest fires are an important source of reactive organic gases and aerosols to the atmosphere....
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